The coherent manipulation of spin and pseudospin underlies existing and emerging quantum technologies, including quantum communication and quantum computation1,2. Valley polarization, associated with ...the occupancy of degenerate, but quantum mechanically distinct valleys in momentum space, closely resembles spin polarization and has been proposed as a pseudospin carrier for the future quantum electronics3,4. Valley exciton polarization has been created in the transition metal dichalcogenide monolayers using excitation by circularly polarized light and has been detected both optically57 and electrically8. In addition, the existence of coherence in the valley pseudospin has been identied experimentally9. The manipulation of such valley coherence has, however, remained out of reach. Here we demonstrate all-optical control of the valley coherence by means of the pseudomagnetic eld associated with the optical Stark eect. Using below-bandgap circularly polarized light, we rotate the valley exciton pseudospin in monolayer WSe2 on the femtosecond timescale. Both the direction and speed of the rotation can be manipulated optically by tuning the dynamic phase of excitons in opposite valleys. This study unveils the possibility of generation, manipulation, and detection of the valley pseudospin by coupling to photons.
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Atomically thin materials such as graphene and monolayer transition metal dichalcogenides (TMDs) exhibit remarkable physical properties resulting from their reduced dimensionality and crystal ...symmetry. The family of semiconducting transition metal dichalcogenides is an especially promising platform for fundamental studies of two-dimensional (2D) systems, with potential applications in optoelectronics and valleytronics due to their direct band gap in the monolayer limit and highly efficient light-matter coupling. A crystal lattice with broken inversion symmetry combined with strong spin-orbit interactions leads to a unique combination of the spin and valley degrees of freedom. In addition, the 2D character of the monolayers and weak dielectric screening from the environment yield a significant enhancement of the Coulomb interaction. The resulting formation of bound electron-hole pairs, or excitons, dominates the optical and spin properties of the material. Here recent progress in understanding of the excitonic properties in monolayer TMDs is reviewed and future challenges are laid out. Discussed are the consequences of the strong direct and exchange Coulomb interaction, exciton light-matter coupling, and influence of finite carrier and electron-hole pair densities on the exciton properties in TMDs. Finally, the impact on valley polarization is described and the tuning of the energies and polarization observed in applied electric and magnetic fields is summarized.
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Single- and few-layer crystals of exfoliated MoTe2 have been characterized spectroscopically by photoluminescence, Raman scattering, and optical absorption measurements. We find that MoTe2 in the ...monolayer limit displays strong photoluminescence. On the basis of complementary optical absorption results, we conclude that monolayer MoTe2 is a direct-gap semiconductor with an optical band gap of 1.10 eV. This new monolayer material extends the spectral range of atomically thin direct-gap materials from the visible to the near-infrared.
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Van der Waals heterostructures are synthetic quantum materials composed of stacks of atomically thin two-dimensional (2D) layers. Because the electrons in the atomically thin 2D layers are exposed to ...layer-to-layer coupling, the properties of van der Waals heterostructures are defined not only by the constituent monolayers, but also by the interactions between the layers. Many fascinating electrical, optical and magnetic properties have recently been reported in different types of van der Waals heterostructures. In this Review, we focus on unique excited-state dynamics in transition metal dichalcogenide (TMDC) heterostructures. TMDC monolayers are the most widely studied 2D semiconductors, featuring prominent exciton states and accessibility to the valley degree of freedom. Many TMDC heterostructures are characterized by a staggered band alignment. This band alignment has profound effects on the evolution of the excited states in heterostructures, including ultrafast charge transfer between the layers, the formation of interlayer excitons, and the existence of long-lived spin and valley polarization in resident carriers. Here we review recent experimental and theoretical efforts to elucidate electron dynamics in TMDC heterostructures, extending from timescales of femtoseconds to microseconds, and comment on the relevance of these effects for potential applications in optoelectronic, valleytronic and spintronic devices.
Electronic and spintronic devices rely on the fact that free charge carriers in solids carry electric charge and spin. There are, however, other properties of charge carriers that might be exploited ...in new families of devices. In particular, if there are two or more minima in the conduction band (or maxima in the valence band) in momentum space, and if it is possible to confine charge carriers in one of these valleys, then it should be possible to make a valleytronic device. Valley polarization, as the selective population of one valley is designated, has been demonstrated using strain and magnetic fields, but neither of these approaches allows dynamic control. Here, we demonstrate that optical pumping with circularly polarized light can achieve complete dynamic valley polarization in monolayer MoS(2) (refs 11, 12), a two-dimensional non-centrosymmetric crystal with direct energy gaps at two valleys. Moreover, this polarization is retained for longer than 1 ns. Our results, and similar results by Zeng et al., demonstrate the viability of optical valley control and suggest the possibility of valley-based electronic and optoelectronic applications in MoS(2) monolayers.
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High-harmonic generation (HHG) in bulk solids permits the exploration of materials in a new regime of strong fields and attosecond timescales1, 2, 3, 4, 5, 6. The generation process has been ...discussed in the context of strongly driven electron dynamics in single-particle bands7, 8, 9, 10, 11, 12, 13, 14. Two-dimensional materials exhibit distinctive electronic properties compared to the bulk that could significantly modify the HHG process15, 16, including different symmetries17, 18, 19, access to individual valleys20, 21 and enhanced many-body interactions22, 23, 24, 25. Here we demonstrate non-perturbative HHG from a monolayer MoS2 crystal, with even and odd harmonics extending to the 13th order. The even orders are predominantly polarized perpendicular to the pump and are compatible with the anomalous transverse intraband current arising from the material's Berry curvature, while the weak parallel component suggests the importance of interband transitions. The odd harmonics exhibit a significant enhancement in efficiency per layer compared to the bulk, which is attributed to correlation effects. The combination of strong many-body Coulomb interactions and widely tunable electronic properties in two-dimensional materials offers a new platform for attosecond physics.
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In recent years, enhanced light-matter interactions through a plethora of dipole-type polaritonic excitations have been observed in two-dimensional (2D) layered materials. In graphene, electrically ...tunable and highly confined plasmon-polaritons were predicted and observed, opening up opportunities for optoelectronics, bio-sensing and other mid-infrared applications. In hexagonal boron nitride, low-loss infrared-active phonon-polaritons exhibit hyperbolic behaviour for some frequencies, allowing for ray-like propagation exhibiting high quality factors and hyperlensing effects. In transition metal dichalcogenides, reduced screening in the 2D limit leads to optically prominent excitons with large binding energy, with these polaritonic modes having been recently observed with scanning near-field optical microscopy. Here, we review recent progress in state-of-the-art experiments, and survey the vast library of polaritonic modes in 2D materials, their optical spectral properties, figures of merit and application space. Taken together, the emerging field of 2D material polaritonics and their hybrids provide enticing avenues for manipulating light-matter interactions across the visible, infrared to terahertz spectral ranges, with new optical control beyond what can be achieved using traditional bulk materials.
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The electronic structure of few-layer graphene (FLG) samples with crystalline order was investigated experimentally by infrared absorption spectroscopy for photon energies ranging from 0.2-1 eV. ...Distinct optical conductivity spectra were observed for different samples having precisely the same number of layers. The different spectra arise from the existence of two stable polytypes of FLG, namely, Bernal (AB) stacking and rhombohedral (ABC) stacking. The observed absorption features, reflecting the underlying symmetry of the two polytypes and the nature of the associated van Hone singularities, were reproduced by explicit calculations within a tight-binding model. The findings demonstrate the pronounced effect of stacking order on the electronic structure of FLG.
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The recent emergence of two-dimensional layered materials -- in particular the transition metal dichalcogenides -- provides a new laboratory for exploring the internal quantum degrees of freedom of ...electrons and their potential for new electronics. These degrees of freedom are the real electron spin, the layer pseudospin, and the valley pseudospin. New methods for the quantum control of the spin and these pseudospins arise from the existence of Berry phase-related physical properties and strong spin-orbit coupling. The former leads to the versatile control of the valley pseudospin, whereas the latter gives rise to an interplay between the spin and the pseudospins. Here, we provide a brief review of both theoretical and experimental advances in this field.
Atomically thin transition metal dichalcogenides are direct-gap semiconductors with strong light-matter and Coulomb interactions. The latter accounts for tightly bound excitons, which dominate their ...optical properties. Besides the optically accessible bright excitons, these systems exhibit a variety of dark excitonic states. They are not visible in the optical spectra, but can strongly influence the coherence lifetime and the linewidth of the emission from bright exciton states. Here, we investigate the microscopic origin of the excitonic coherence lifetime in two representative materials (WS
and MoSe
) through a study combining microscopic theory with spectroscopic measurements. We show that the excitonic coherence lifetime is determined by phonon-induced intravalley scattering and intervalley scattering into dark excitonic states. In particular, in WS
, we identify exciton relaxation processes involving phonon emission into lower-lying dark states that are operative at all temperatures.
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